Individual aerosol particles from biomass burning in southern Africa: 2. Compositions and aging of inorganic particles

Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field- emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen-bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass- burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes

Atmospheric tar balls: Particles from biomass and biofuel burning

"Tar balls'' are amorphous, carbonaceous spherules that occur in the tropospheric aerosol as a result of biomass and biofuel burning. They form a distinct group of particles with diameters typically between 30 and 500 nm and readily identifiable with electron microscopy. Their lack of a turbostratic microstructure distinguishes them from soot, and their morphology and composition (similar to90 mol % carbon) renders them distinct from other carbonaceous particles. Tar balls are particularly abundant in slightly aged (minutes to hours old) biomass smoke, indicating that they likely form by gas-to-particle conversion within smoke plumes. The material of tar balls is initially hygroscopic; however, the particles become largely insoluble as a result of free radical polymerization of their organic molecules. Consequently, tar balls are primarily externally mixed with other particle types, and they do not appreciably increase in size during aging. When tar balls coagulate with water-bearing particles, their material may partly dissolve and no longer be recognizable as distinct particles. Tar balls may contain organic compounds that absorb sunlight. They are an important, previously unrecognized type of carbonaceous (organic) atmospheric particle

Individual aerosol particles from biomass burning in southern Africa: 1. Compositions and size distributions of carbonaceous particles

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy ( TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic ( K- salt) inclusions, " tar ball'' particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged ( similar to 1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/ sulfate and soot/ sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/ sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea- salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles

Modelling the spring ozone maximum and the interhemispheric asymmetry in the remote marine boundary layer 1. Comparison with surface and ozonesonde measurements

Here we report a modelling study of the spring ozone maximum and its interhemispheric asymmetry in the remote marine boundary layer (MBL). The modelled results are examined at the surface and on a series of time-height cross sections at several locations spread over the Atlantic, the Indian, and the Pacific Oceans. Comparison of model with surface measurements at remote MBL stations indicate a close agreement. The most striking feature of the hemispheric spring ozone maximum in the MBL can be most easily identified at the NH sites of Westman Island, Bermuda, and Mauna Loa, and at the SH site of Samoa. Modelled ozone vertical distributions in the troposphere are compared with ozone profiles. For the Atlantic and the Indian sites, the model generally produces a hemispheric spring ozone maximum close to those of the measurements. The model also produces a spring ozone maximum in the northeastern and tropical north Pacific close to those measurements, and at sites in the NH high latitudes. The good agreement between model and measurements indicate that the model can reproduce the proposed mechanisms responsible for producing the spring ozone maximum in these regions of the MBL, lending confidence in the use of the model to investigate MBL ozone chemistry (see part 2 and part 3). The spring ozone maximum in the tropical central south Pacific and eastern equatorial Pacific are less well reproduced by the model, indicating that both the transport of $O_3$ precursors from biomass burning emissions taking place in southeastern Asia, Australia, Oceania, southern Africa, and South America are not well represented in the model in these regions. Overall, the model produces a better simulation at sites where the stratosphere and biomass burning emissions are the major contributors.Comment: 24 pages, 8 figure

Influence of southern hemispheric biomass burning on midtropospheric distributions of nonmethane hydrocarbons and selected halocarbons over the remote South Pacific

Aircraft measurements of nonmethane hydrocarbons (NMHCs) and halocarbons were made over the remote South Pacific Ocean during late August-early October 1996 for NASA's Global Tropospheric Experiment (GTE) Pacific Exploratory Mission-Tropics A (PEM-Tropics A). This paper discusses the large-scale spatial distributions of selected trace gases encountered during PEM-Tropics A. The PEM-Tropics A observations are compared to measurements made over the southwestern pacific in early November 1995 as part of Aerosol Characterization Experiment (ACE 1). Continental pollution in the form of layers containing elevated levels of O3 was observed during a majority of PEM-Tropics flights, as well as during several ACE 1 flights. The chemical composition of these air masses indicates that they were not fresh and were derived from nonurban combustion sources. The substantial impact of biomass burning on the vertical structure of the South Pacific troposphere is discussed. Copyright 1999 by the American Geophysical Union

Impacts of biomass burning in Southeast Asia on ozone and reactive nitrogen over the western Pacific in spring

Aircraft measurements of ozone (O3) and its precursors (reactive nitrogen, CO, nonmethane hydrocarbons) were made over the western Pacific during the Transport and Chemical Evolution Over the Pacific (TRACE-P) campaign, which was conducted during February-April 2001. Biomass burning activity was high over Southeast Asia (SEA) during this period (dry season), and convective activity over SEA frequently transported air from the boundary layer to the free troposphere, followed by eastward transport to the sampling region over the western Pacific south of 30°N. This data set allows for systematic investigations of the chemical and physical processes in the outflow from SEA. Methyl chloride (CH3Cl) and CO are chosen as primary and secondary tracers, respectively, to gauge the degree of the impact of emissions of trace species from biomass burning. Biomass burning is found to be a major source of reactive nitrogen (NO x, PAN, HNO3, and nitrate) and O3 in this region from correlations of these species with the tracers. Changes in the abundance of reactive nitrogen during upward transport are quantified from the altitude change of the slopes of the correlations of these species with CO. NOx decreased with altitude due to its oxidation to HNO3. On the other hand, PAN was conserved during transport from the lower to the middle troposphere, consistent with its low water solubility and chemical stability at low temperatures. Large losses of HNO3 and nitrate, which are highly water soluble, occurred in the free troposphere, most likely due to wet removal by precipitation. This has been shown to be the major pathway of NOy loss in the middle troposphere. Increases in the mixing ratios of O3 and its precursors due to biomass burning in SEA are estimated using the tracers. Enhancements of CO and total reactive nitrogen (NOy), which are directly emitted from biomass burning, were largest at 2-4 km. At this altitude the increases in NOy and O3 were 810 parts per trillion by volume (pptv) and 26 parts per billion by volume (ppbv) above their background values of 240 pptv and 31 ppbv, respectively. The slope of the O3-CO correlation in biomass burning plumes was similar to those observed in fire plumes in northern Australia, Africa, and Canada. The O3 production efficiency (OPE) derived from the O3-CO slope and NOx/CO emission ratio (ER) is shown to be positively correlated with the C2H4 /NOx ER, indicating that the C2H4/NO x ER is a critical parameter in determining the OPE. Comparison of the net O3 flux across the western Pacific region and total O3 production due to biomass burning in SEA suggests that about 70% of O3 produced was transported to the western Pacific. Copyright 2004 by the American Geophysical Union

The AMMA mulid network for aerosol characterization in West Africa

Three ground based portable low power consumption microlidars (MULID) have been built and deployed at three remote sites in Banizoumbou (Niger), Cinzana (Mali) and M'Bour (Senegal) in the framework of the African Monsoon Multidisciplinary Analyses (AMMA) project for the characterization of aerosols optical properties. A description of the instrument and a discussion of the data inversion method, including a careful analysis of measurement uncertainties (systematic and statistical errors) are presented. Some case studies of typical lidar profiles observed over the Banizoumbou site during 2006 are shown and discussed with respect to the AERONET 7-day back-trajectories and the biomass burning emissions from the Combustion Emission database for the AMMA campaign